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Charley was born on April 15, 1912, the day the Titanic sank, and first appears in the play Storm Warning (2001). Storm takes place in 1930, making her 18 years old at the time.

She is born into a well-to-do family; her mother is Lady Louisa Pollard and two sisters, Margaret and Cecelia, are mentioned. Charley and her siblings grow up in a manor house in Hampshire, looked after by servants. However, Charley rebels against this existence and, styling herself an Edwardian adventuress, runs away from home seeking excitement. Making an appointment to meet a young man in Singapore on New Year's Day 1931, she stows away on board the Airship R101 disguised as a male member of the crew. There, she meets the Doctor and together they discover the secret mission the airship is on. At the conclusion of the story, she is rescued from the fated crash of the R101 by the Doctor and taken on board the TARDIS as his newest companion.

There are consequences to the Doctor taking Charley on board, however. According to history, Charley was supposed to die in the R101 crash and the Doctor's rescue of her causes a temporal paradox. After a while, the Web of Time begins to break down as anachronisms seep into history and "anti-time" starts to infect the universe, with Charley as both focus and gateway. The Time Lords of Gallifrey take notice, and Lord President Romana gives orders to arrest Charley and the Doctor. Charley is willing to sacrifice herself to save the universe, but the Doctor is unable to sacrifice her, taking the forces of anti-time into himself instead. History is then altered so that the paradox of Charley's continued existence became part of established history – in other words, the paradox and the resulting consequences, including the change in the timeline, were supposed to happen.

However, having absorbed anti-time, the Doctor now is a danger to the universe, and so has to exile himself into a parallel universe where time does not exist. He intended to do so alone, but Charley stows away aboard the TARDIS and follows him into exile. Eventually, the Doctor discovers he is free of the anti-time infection and he and Charley manage to find their way back, accompanied by C'rizz, a native of that other universe.

It is the later death of C'rizz that prompts her decision to leave the TARDIS. She quickly changes her mind, but due to a series of events involving Cybermen, temporal shifts and memory loss, parts company with the Doctor. While he believes she has voluntarily left him, Charley actually ends up marooned on an island in the year 500002, believing that the Doctor had died in their confrontation with the Cybermen. She builds a makeshift crystal telegraph and sends an SOS repeatedly into space, hoping that anyone, particularly the Doctor, would rescue her. When her message is finally answered, it turned out to be the Sixth Doctor who saves her. Charley chose to continue traveling with this earlier incarnation, keeping the circumstances of her past and his future a secret from him. This leads the Doctor to grow suspicious of her secrecy and poorly devised lies.

Eventually she runs afoul of a secret TARDIS inhabitant named Mila, who swaps places with her. Charley is infected with a virus rendering her invisible and non-corporeal while Mila pretends to be her. Of the dozens of companions Mila has secretly encountered, Charley is the only one she could infect, because she's the only companion the TARDIS refused to protect from infections. It is implied that the TARDIS hates Charley, because of her multiple temporal paradoxes. Charley is cured by the mysterious Viyrans and she spends years helping in their mission to rid the universe of certain viruses. Finally she finds the Sixth Doctor again, still traveling with Mila who is still pretending to be Charley. But Mila dies saving the Doctor's life and Charley takes the opportunity to finally set the Web of Time straight. She asks the Viyrans to alter the Doctor's memories so that all the adventures they shared would be remembered with Mila's name and true appearance. This way, years later, when the Eighth Doctor meets Charley, he'll believe it to be their first encounter. What happens to Charley after she leaves the Sixth Doctor is unclear, but it seems she continues to work for the Viyrans.

Charley's exuberant personality matched the Eighth Doctor's well. She embraced the wonders of the universe that travel with the Doctor showed her and helped the Doctor fight the evils he encountered with courage. She was not only loyal to the Doctor, but also developed romantic feelings for him and eventually confessed them. The Doctor was very fond of Charley, and admitted later that she was his friend and he loved her, but what that meant for a virtually immortal Time Lord was unclear, as the relationship between the two was not a physical one.

In the third issue of the ongoing Doctor Who comic book series from IDW Publishing (2009), Charley is mentioned by the Shadow Architect and the Tenth Doctor as an instance where the Doctor has interfered with a static point in time.

In the bonus tracks to the Companion Chronicle Solitaire, it was revealed that Charley will (at some point in the future) get her own series picking up from the events of Blue Forgotten Planet.

Before regenerating into the War Doctor in The Night of the Doctor, the Eighth Doctor mentions Charley, marking the first time that any of the Big Finish audio series has been directly referenced in the television show.[2]